arXiv subjects

Jérôme Palaudoux

Publications and source records attributed to Jérôme Palaudoux.

3 recordsLinked to original sources

arXiv2021

Specific chemical bond relaxation unravelled by analysis of shake-up satellites in the oxygen single site double core hole spectrum of CO$_2$

We developed recently [A. Ferté, et al., J. Phys. Chem. Lett. 11, 4359 (2020)] a method to compute single site double core hole (ssDCH or K$^{-2}$) spectra. We refer to that method as NOTA+CIPSI. In the present paper this method is applied to the O K$^{-2}$ spectrum of the CO$_2$ molecule, and we use this as an example to discuss in detail its convergence properties. Using this approach, a theoretical spectra in excellent agreement with the experimental one is obtained. Thanks to a thorough interpretation of the shake-up states responsible for the main satellite peaks and with the help of a comparison with the O K$^{-2}$ spectrum of CO, we can highlight the clear signature of the two non equivalent carbon oxygen bonds in the oxygen ssDCH CO$_2$ dication.

physics.chem-ph↗

arXiv2019

Time-resolved inner-shell photoelectron spectroscopy: from a bound molecule to an isolated atom

Due to its element- and site-specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH$_3$I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

physics.chem-ph↗

arXiv2017

Coulomb explosion imaging of concurrent CH$_{2}$BrI photodissociation dynamics

The dynamics following laser-induced molecular photodissociation of gas-phase CH$_{2}$BrI at 271.6 nm were investigated by time-resolved Coulomb explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH$_{2}$BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH$_{2}$Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb explosion imaging as a real-time probe of chemical dynamics.

physics.chem-ph↗